Decreasing carbon emissions by replacing Portland cement (PC) with supplementary cementitious materials (SCMs), such as low-grade limestone (LS) and calcined clays (CC), has tremendous potential for stabilization/solidification (S/S) of industrial hazardous waste primarily with heavy metals. Recently, a low-carbon-based cementitious binder, namely, limestone calcined clay cement (LC), has emerged as an alternative for S/S treatment of wastes. However, comprehensive comparison between LC and PC application in solidifying/stabilizing wastes has not been conducted. This study aims to investigate the S/S efficiency of Pb- Zn smelter residue (LZSR) comprising heavy metals lead (Pb), zinc (Zn), and cadmium ( Cd) at higher concentrations. LZSR is treated with LC and PC for capturing strength and leaching toxicity. The test results indicate that low-grade CC and LS in the LC binder can promote the alkaline environment, and act as fillers in solidifying heavy metals. The toxicity characteristic leaching procedure leaching concentrations of untreated ( UT) LZSR were 503 mg/kg, 1266 mg/ kg, and 251 mg/kg for Pb, Zn, and Cd, respectively. After a 28-day curing, the leaching concentrations in LC-treated LZSR reduced to 4.33 mg/kg, 189.68 mg/ kg, and 0.46 mg/kg, while the leaching concentrations of PC-treated LZSR reduced to 29 mg/kg, 338 mg/kg, and 6 mg/kg for Pb, Zn, and Cd, respectively. The maximum immobilization efficiencies for Pb, Zn, and Cd reached 85%, 99%, and 99%, respectively. Moreover, the insoluble phases for Pb, Zn, and Cd obtained from the sequential extraction test results were 63.5%, 72.1%, and 42.4% for LC-treated LZSR and 35.7%, 38%, and 43% for PCtreated LZSR with binder content of 8% binder and curing time of 28 days. Increasing curing time and binder content reduced leaching concentrations, and the underneath mechanisms were interpreted by XRD, SEM-EDS, and FTIR analyses. Overall, the results indicate that Pb, Zn, and Cd can be successfully immobilized using 8% LC binder by transforming soluble heavy metals to insoluble hydroxides and their complexes.